Aqueous electrolyte design is pivotal for boosting the energy density and lifespan of aqueous batteries, because it can expand the electrochemical stability window and also mitigate the parasitic side reactions. Until now, three main kinds of electrolytes, i.e., water-in-salt, eutectic, and additives-modified electrolytes, have been developed by which the activity of H2O can be lowered and/or the formed specific solid–electrolyte interphase (SEI) can mitigate the decomposition of H2O. However, there is still a lack of a universal model to elucidate the reason for the improved performance, especially as the SEI interpretation becomes ever more controversial. Herein, we present a quantitative and graphical model of the electrolyte solvation structure and metal-ion (de)solvation process (i.e., interfacial model) to summarize a relationship between the electrolyte–electrode interfacial chemistry and electrode performance. This Focus Review extends the solvation structure and interfacial model into the field of aqueous electrolytes, revealing the essential influence of the solvation structure’s properties on electrolyte stability and electrode performance, by which electrode performance and electrolyte design can be more quantitatively and accurately understood.
|Original language||English (US)|
|Number of pages||20|
|Journal||ACS Energy Letters|
|State||Published - Jan 23 2023|
Bibliographical noteKAUST Repository Item: Exported on 2023-01-30
Acknowledgements: The authors greatly thank the National Natural Science Foundation of China (22122904) for funding support. This work is also supported by the National Natural Science Foundation of China (21978281, 11974150, 22109155) and the Fundamental Research Funds for the Central Universities (lzujbky-2021-pd10). The authors also thank the bureau of international cooperation Chinese academy of sciences, CAS-NST Joint Research Projects (121522KYSB20200047), and the Scientific and Technological Developing Project of Jilin Province (YDZJ202101ZYTS022). The computational work was done on the KAUST supercomputer. This work was also supported by Hanyang University.
This publication acknowledges KAUST support, but has no KAUST affiliated authors.